Abstract:
The selective electrochemical reduction of CO2 in the CO2 reduction reaction (CO2RR) is a crucial strategy for storing energy from intermittent sources in the form of chemical bonds (e.g. solar fuels) and as a pathway to converting CO2 in industrial waste streams to value-added products. State-of-the-art solid-state catalysts produce useful products, but typically do so non-selectively with H2 production from competitive water reduction. Alternatively, molecular catalysts show promise for the selective reduction of CO2 to single products, but usually perform with lower activity compared to their solid-state analogues. My research group is focused on the development of new catalytic systems for the CO2RR that operate with the selectivity of molecular catalysts but the activity of solid-state catalysts. In this talk, I will present some of our work using polymer encapsulation to increase the catalytic activity and selectivity of molecular catalyst for the CO2RR. In particular, we show that encapsulating cobalt phthalocyanine within a coordinating polyvinylpyridine polymer leads to a dramatic enhancement in its activity and selectivity for the CO2RR in aqueous phosphate solution. Using a combination of electroanalytical studies and in situ electrochemical X-ray absorbance measurements, we demonstrate that the encapsulating polymer modulates all coordination spheres surrounding the catalyst active site, and that this has a profound impact on the catalytic performance and mechanism.
Biography:
Professor Charles C. L. McCrory earned undergraduate degrees in chemistry and mathematics from Indiana University working with Prof. George Ewing conducting spectroscopic studies of thin film water composition and structure on single-crystal surfaces. He attended Stanford University for his Ph.D. in Chemistry where he worked with Prof. Christopher Chidsey to understand the kinetics and mechanisms of electrocatalytic oxygen reduction and alcohol oxidation by discrete molecular complexes immobilized onto carbon surfaces. He conducted Postdoctoral research with Jonas Peters at Caltech where he studied electrocatalytic hydrogen evolution using molecular cobalt and nickel complexes. In 2011, Prof. McCrory joined the research staff of the Joint Center for Artificial Photosynthesis (JCAP), a DOE Energy Innovation Hub, where supervised a research team developing and implementing benchmarking protocols for heterogeneous water splitting catalysts. He joined the faculty at the University of Michigan in 2015, where he is currently an Associate Professor of Chemistry and Associate Professor of Macromolecular Science & Engineering. His current work focuses on the study of the mechanisms and kinetics of electrocatalytic transformations of small molecules for energy storage and environmental remediation. His work has been recognized by several awards including an NSF CAREER Award, a DOE Early Career Award, and a Cottrell Scholars Award.